The effect of alkali metal chlorides on the viscoelastic behavior and yielding properties of silica suspensions was studied through creep-recovery and dynamic oscillatory tests with stress control. Then, the viscoelasticity of the pulps was correlated with the silica zeta potential, aggregate size, and the percentage of cations adsorbed on the surface of the ore. The results indicate that larger cations are more prone to adhere to the silica surface, which increases the number of ionic bonds that bind the particles. This generates stronger particle networks and a greater agglomeration of particles, especially those smaller than 10 µm. As the size of the bare cations increases, the rheological response provides higher values of yield stress, complex viscosity, and viscoelastic moduli, but in turn, pulps undergo minor deformations under the application of stress. Dynamic oscillatory tests suggest structural changes, with the phase angle following the inverse relationship with the bare cation size, indicating that the liquid-like character of the pulps increases as the size of the cations increases.Minerals 2019, 9, 216 2 of 15 water that surrounds them. Small ions such as Li + are known as maker ions because they attract water molecules more strongly than water molecules do to each other, forming a layer of structured water around the ions. On the other hand, large ions such as Cs + are known as breakers; they interact weakly with water, generating a layer of structureless water around them. This implies that the hydrated size of ions in solution follows the trend Li + > Na + > K + , which is opposite to the bare ion size.More than a century ago, Hofmeister related the precipitation of proteins with the size of bare ions in solution [8]; interestingly, the order established by Hofmeister has been found in various systems, such as colloidal suspensions of tungsten trioxide, magnetite, alumina, titanium, hematite, and silica [9][10][11][12][13]. Here, we focus on silica, which has been studied extensively due to its relevance in numerous industrial applications [14-16]; however, it has not been studied combining rheological and physicochemical results in the presence of a series of alkali metal chloride salts. A particularly important result for our work is that of Franks [9], who measured the zeta potential and yield stress of quartz suspensions in concentrated solutions of monovalent electrolytes, finding that poorly hydrated ions, such as Cs + and K + , have a greater impact in reducing the absolute value of the zeta potential than highly hydrated ions, such as Li + and Na + . Franks found a higher yield stress when the pulp was in the presence of breaker ions, although the results were highly dependent on the pH. A challenge that is not yet fully resolved is that of high isoelectric point minerals, such as alumina, the properties of which follow a trend with the size of ions opposite to silica; for example, maker ions generate stronger alumina networks [17][18][19][20][21]. Parson et al. [19] developed a Poisson...